CN104593803B - A kind of Driven by Solar Energy high-temperature electrolysis CO 2/ H 2o preparing synthetic gas system and application thereof - Google Patents
A kind of Driven by Solar Energy high-temperature electrolysis CO 2/ H 2o preparing synthetic gas system and application thereof Download PDFInfo
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Abstract
The present invention relates to a kind of Driven by Solar Energy high-temperature electrolysis CO
2/ H
2o preparing synthetic gas system, this system comprises electrolysis cells and photo-thermal unit, and electrolysis cells is made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen, and photovoltaic element converts solar energy into electrical energy, and provides required electrolysis voltage or electric current; Photo-thermal unit converts solar energy into heat energy, carries out heating and makes it reach molten state, and heat electrolyzer to electrolysis temperature to solid state electrolyte; Ionogen is mixed type fused electrolyte.This system utilizes the collaborative coupling of the heat/electricity of solar energy-Re-electrochemical couple process, constitute perfect green solar to transform and stocking system, there is clean, safe and continuable feature, for the comprehensive utilization of energy-saving and emission-reduction and solar energy resources provides new approach, under achieving low electrolysis voltage and relative low temperature condition simultaneously, CO
2/ H
2the common converting preparing synthetic gas of O, energy-conservation, realize CO efficiently
2recycling.
Description
Technical field
The present invention relates to one and utilize new forms of energy Driven by Solar Energy CO
2/ H
2o transforms preparing synthetic gas system and application thereof, belongs to Solar use, energy-saving and emission-reduction and CO
2resource utilization field.
Background technology
CO
2one of topmost greenhouse gases causing Global climate change.CO
2a large amount of discharges become one the international problem of great effect produced to the change of future world general layout, how control CO
2discharge be put into the primary subject under discussion of national governments, United Nations's meeting, become strategic problem urgently to be resolved hurrily in global many significant problems, add that carbonic acid gas is potential carbon resource, therefore develop corresponding carbon dioxide recovery and utilize technology to have important strategic importance.The recovery of current carbonic acid gas transforms and mainly concentrates on catalytic activation synthesis organic-fuel or industrial chemicals, as CH
4, CO+H
2, methyl alcohol etc.Research group of Tokyo polytechnical university one developed a kind of NEW TYPE OF COMPOSITE photocatalyst in 2008, and sunlight can be utilized CO
2be converted into CO, this method is normal-temperature light catalysis method, and phototransformation rate is extremely low; Northeastern Japan Utilities Electric Co. for catalyzer, can make carbonic acid gas mix with under pressure in certain temperature with hydrogen with rhodium-magnesium, generates methane; Toshiba Corp directly mixes with the acetylene taking hydrogen as substrate with setting off gas, utilizes electron beam or laser beam energizes, methanol and CO.But these reaction needed are in High Temperature High Pressure and just can carry out under having catalyzer existent condition, need to be equipped with special reactor, reaction process needs to consume a large amount of energy and power, in addition the performance of catalyzer is lower, easy inactivation under high temperature, therefore utilizes the extensive trans-utilization carbonic acid gas of this high-pressure catalytic hydride process to also have a lot of difficulty.Compared to the chemical process needing high-temperature and high-pressure conditions comparatively harsh, in recent years, the comparatively gentle and electrochemistry fixation of C O of easy handling of reaction conditions
2technology becomes CO
2one of focus of resource utilization area research.Current CO
2electrochemical reduction research is mainly by CO
2be dissolved in the organic solvent of water solvent and non-water, but this also limit its industrial applications simultaneously, CO in addition
2for gas molecule, Direct Electrolysis reduction is very difficult, and one is need high energy consumption (high electrolysis voltage), and two is that electrolytic reaction is very complicated, efficiency and poor selectivity.Based on this, develop a kind of low cost, simple, the efficient CO of device
2the method of recycling, with device, just seems extremely important in the hope of better economy, society and environmental benefit.
Summary of the invention
The invention provides that a kind of system is simple, energy-conservation, low cost, efficiently CO
2resource utilization method, with CO
2recycling is target, is intended to the synergistic effect utilizing solar energy optical-thermal/photoelectricity, by CO
2/ H
2o electrolysis coupling reduction under high-temperature molten salt condition is synthetic gas, achieves sun power to chemical transformation of energy and storage simultaneously.Achieve under low electrolysis voltage and relative low temperature condition, CO simultaneously
2/ H
2the common converting preparing synthetic gas of O, and electrolytic reaction is relatively simple, good reaction selectivity.
The object of the invention is to be achieved through the following technical solutions:
A kind of Driven by Solar Energy high-temperature electrolysis CO
2/ H
2o preparing synthetic gas system, this system comprises electrolysis cells and photo-thermal unit, electrolysis cells is made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen, it is characterized in that: the photovoltaic element of described electrolysis cells converts solar energy into electrical energy, and provides required electrolysis voltage or electric current; Described photo-thermal unit converts solar energy into heat energy, carries out heating and makes it reach molten state, and heat electrolyzer to electrolysis temperature to solid state electrolyte; Described ionogen is the mixture of fused carbonate and fusible hydrate, or the mixture of fused carbonate and molten oxide, or the mixture of fused carbonate, fusible hydrate and molten oxide, in electrolysis, at [1A, 3A) in interval, electrolyzer temperature is more than 600 DEG C, the CO in electrolyte absorption air
2/ H
2o is regenerated; Preferably, Faradaic current is 1A-2A, and electrolyzer temperature is 600 DEG C-800 DEG C; When ionogen is the mixture of fused carbonate and fusible hydrate, mol ratio is carbonate: oxyhydroxide=1:0.5 ~ 1; When ionogen is the mixture of fused carbonate and molten oxide, mol ratio is carbonate: oxide compound=1:0.5 ~ 1; When ionogen is the mixture of fused carbonate, fusible hydrate and molten oxide, mol ratio is carbonate: (oxyhydroxide+oxide compound)=1:0.5 ~ 1.；
Further, one in solar cell, nano-crystalline solar battery, dye-sensitized solar battery and concentrating solar battery that described photovoltaic element adopts silicon solar cell plate, multi-band-gap solar cell, functional high molecule material to prepare, or the two or more serial or parallel connection combination in above-mentioned solar cell types; Silicon solar cell plate can adopt silicon single crystal, polysilicon, non-crystalline silicon, and multi-band-gap solar cell can adopt the multi-element compounds such as gallium arsenide III-V compound, Cadmium Sulfide, copper indium diselenide to be material;
Further, described photo-thermal unit adopts one or more the combination in Fresnel Lenses, reflection-type beam condenser, refraction type light gathering device, small-sized groove type line-focusing system, dish-style system or tower system, regulates and controls Heating temperature by regulating spot size or focusing ratio;
Further, the cathode material of described electrolysis cells is nickel, platinum, titanium, ruthenium, iridium, palladium, iron, tungsten, chromium, copper, gold, graphite or stainless steel, or the alloy of several formation in above-mentioned materials;
Further, the anode material of described electrolysis cells is nickel, platinum, titanium, ruthenium, iridium, palladium, iron, tungsten, chromium, copper, gold, graphite or stainless steel, or the alloy of several formation in above-mentioned materials;
Further, described electrolyzer adopts high temperature corrosion-resisting type reactor;
Further, carbonate is Li
2cO
3, Na
2cO
3, K
2cO
3, Rb
2cO
3, MgCO
3, CaCO
3, SrCO
3, BaCO
3, ZnCO
3, Li
2siO
3, Na
2siO
3, K
2siO
3, Rb
2siO
3in one or more mixture; Oxyhydroxide is LiOH, NaOH, KOH, RbOH, Mg (OH)
2, Ca (OH)
2, Sr (OH)
2, Ba (OH)
2, Zn (OH)
2in one or more mixture; Oxide compound is Li
2o, Na
2o, K
2o, Rb
2o, MgO, CaO, SrO, BaO, ZnO, SiO
2, Al
2o
3, Fe
2o
3in one or more mixture.
Based on above-mentioned Driven by Solar Energy high-temperature electrolysis CO
2/ H
2the high-temperature electrolysis CO of O preparing synthetic gas system
2/ H
2the method of O preparing synthetic gas, is characterized in that: the method comprises the steps:
(1) electrolysis cells be made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen is built;
(2) solid state electrolyte is added in thermal electrolysis to form molten state ionogen by photo-thermal unit;
(3) electrolyzer homo(io)thermism is controlled at 600 DEG C-800 DEG C;
(4) in electrolyzer, CO is passed into by airway
2and H
2o, controls direct supply current constant at 1A-2A, reaction 1h-2h, and main reaction one step generates primary product synthetic gas CO and H
2, main reaction is: CO
2+ H
2o=CO+H
2+ O
2, the intermediate product carbon simple substance that side reaction obtains and hydrogen, side reaction is:
1) Formed simple substance the CO that reduces
2/ H
2o generates CO/H
2:
CO
2＝C+O
2
C+CO
2＝2CO
C+H
2O＝H
2+CO
2) water electrolysis generates H
2, H
2reduction CO
2generate CO
H
2O＝H
2+1/2O
2
H
2+CO
2＝CO+H
2O；
Its electrolytic reaction mechanism is:
Anode: 2O
2--4e
-=O
2
Negative electrode: 2OH
-+ CO
3 2-+ 4e
-=CO+H
2+ 4O
2-
2H
++CO
3 2-+4e
-＝CO+H
2+2O
2-。
Advantageous Effects of the present invention is as follows:
1, the present invention utilizes new forms of energy sun power by CO
2/ H
2o synergy transforms preparing synthetic gas (H
2and CO), the method utilizes solar energy-Re-electrochemical couple (solarthermalelectrochemicalproduction, be called for short STEP) process heat/electricity work in coordination with coupling, collaborative coupling regulation and control solar energy-Re-electric utilising efficiency and molecule light-Re-electrochemical reaction characteristic, the heat energy that the photo-thermal of sun power and photovoltaic effect are produced and electric energy, act synergistically on the ionogen be made up of oxide compound, carbonate, oxyhydroxide or its mixture, carry out specific CO
2/ H
2o chemical conversion preparing synthetic gas reacts, and is transformed by sun power and saves as chemical energy, realizing CO simultaneously
2effective utilization of resource utilization.
2, electrolytic reaction process, converts solar energy into heat energy by photo-thermal unit, heating ionogen, according to electrolytical difference regulation and control Heating temperature; Use sun power to provide electric energy, according to electrolytical kind and Heating temperature, the electrolysis voltage needed for regulation and control or electric current, by electrolysis CO simultaneously
2/ H
2o, obtains H at negative electrode
2and CO, anode obtains O
2, achieve sun power to chemical transformation of energy and storage, the CO in electrolytic process in electrolyte absorption air
2/ H
2o, makes ionogen be regenerated, thus achieves CO
2recycle and recycling.
3, high-temperature molten salt system majority is in the past single mixed melting carbonate, CO
2/ H
2the common electrolysis temperature of O is all more than 800 DEG C, and the present invention adds a certain proportion of oxyhydroxide and/or oxide compound innovatively on the basis of carbonate.Oxyhydroxide both as the source of protium, can also reduce the fusing point of whole fused salt mixt system simultaneously, made CO
2/ H
2o can realize electrolysis at a lower temperature.Oxide compound, after reaching molten state, can absorb the CO in air
2and H
2o, is converted into carbonate and oxyhydroxide, plays the effect similar with carbonate, hydroxide mixture, also makes CO
2/ H
2o can realize electrolysis at a lower temperature, achieves CO energy-efficiently
2recycling.For sodium salt, as shown in Figure 1:
Absorb: Na
2o+CO
2=Na
2cO
3
Na
2O+H
2O＝2NaOH
Release: Na
2cO
3=Na
2o+CO
2
2NaOH＝Na
2O+H
2O
4, the invention has the advantages that a step generates synthetic gas (H
2and CO), main reaction is: CO
2+ H
2o=CO+H
2+ O
2, the intermediate product carbon simple substance that side reaction obtains and hydrogen, side reaction is:
1) Formed simple substance the CO that reduces
2/ H
2o generates CO/H
2:
CO
2＝C+O
2
C+CO
2＝2CO
C+H
2O＝H
2+CO
2) water electrolysis generates H
2, H
2reduction CO
2generate CO
H
2O＝H
2+1/2O
2
H
2+CO
2＝CO+H
2O；
5, the present invention works in coordination with the photo-thermal/photoelectric coupling effect utilizing sun power, and secondary electrochemical effect, builds efficient integrated coupled mode CO
2/ H
2o transforms preparing synthetic gas system, and a step generates primary product H
2with CO and a small amount of by-product solid simple substance carbon.This system capacity is all from sun power, make use of solar energy optical-thermal, photoelectricity two portions in phase simultaneously, constitute perfect green solar to transform and stocking system, there is clean, safe and continuable feature, for the comprehensive utilization of energy-saving and emission-reduction and solar energy resources provides new approach.
Accompanying drawing explanation
Fig. 1 present system schematic diagram;
Fig. 2 present system schematic diagram;
In figure: 1 anode; 2 electrolyzers; 3 ionogen; 4 negative electrodes; 5 airways; 6 anodic product O
2; 7 reaction raw materials CO
2/ H
2o; 8 cathode product CO/H
2; 9 varistors; 10 solar panels; 11 wires; 12 condensing apparatuss.
Embodiment
Below in conjunction with accompanying drawing, the invention will be further described.
The present invention is based on high-temperature electrolysis CO
2/ H
2o preparing synthetic gas system, as shown in Figure 2, this system comprises electrolysis cells and photo-thermal unit, electrolysis cells is made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen, the negative electrode of electrolysis cells and anode are placed in same electrolyzer, photovoltaic element converts solar energy into electrical energy, and provides required electrolysis voltage or electric current; Photo-thermal unit heats the ionogen in electrolyzer, passes into CO by airway in electrolyzer
2and H
2o, and derive cathode product CO and H by respective airway
2and anodic product O
2.Described photo-thermal unit converts solar energy into heat energy, carries out heating and makes it reach molten state, and heat electrolyzer to electrolysis temperature to solid state electrolyte, regulates and controls Heating temperature by regulating spot size or focusing ratio; Described ionogen is the mixture of fused carbonate and fusible hydrate, or the mixture of fused carbonate and molten oxide, or the mixture of fused carbonate, fusible hydrate and molten oxide, in electrolysis, in (0A-3A) interval, electrolyzer temperature is more than 600 DEG C, the CO in electrolyte absorption air
2/ H
2o is regenerated; When electric current is less than 1A, productive rate crosses low reaction comparatively slowly, and when electric current is greater than 2A, react violent electrode corrosion seriously, yield poorly, therefore the preferred 1A-2A of electric current, preferably, Faradaic current is 1A-2A, and electrolyzer temperature is 600 DEG C-800 DEG C; By the adjustment regulating Faradaic current and ionogen composition to realize production concentration.
Embodiment 1
Respectively by 20gLi
2cO
3, 20gNa
2cO
3, 20gK
2cO
3grind in mortar with 45.09gKOH and mix, be transferred in corundum crucible; Be 30cm by surface-area respectively
2nickel sheet and iron wire as anode and negative electrode, reaction do not limit by electrode area size, and area larger to react favourable; The spot size of Fresnel Lenses is regulated to make homo(io)thermism be 650 DEG C; The varistor of solar panel circuit is regulated to make current constant be 2A.React after 1 hour, in the gas of generation, synthetic gas content (volume percent) is: 89.72%H
2, 6.857%CO.
Embodiment 2
Respectively by 20gLi
2cO
3, 20gNa
2cO
3, 20gK
2cO
3with 51.63gBa (OH)
2grind in mortar and mix, be transferred in corundum crucible; Be 20cm by surface-area respectively
2nichrome wire and iron wire as anode and negative electrode; The focusing ratio of accommodation reflex formula condensing apparatus makes homo(io)thermism be 750 DEG C; The varistor of solar panel circuit is regulated to make current constant be 2A.React after 1 hour, in the gas of generation, synthetic gas content (volume percent) is: 85.67%H
2, 6.03%CO.
Embodiment 3
Respectively by 30gLi
2cO
3, 30gNa
2cO
3, 30gBaCO
3, 10.18gLiOH and 33.91gZnO grind and mix in mortar, is transferred in high purity nickel reactor; Be 15cm by surface-area respectively
2nickel sheet and nickel wire as anode and negative electrode; The spot size of Fresnel Lenses is regulated to make homo(io)thermism be 600 DEG C; The varistor of solar panel circuit is regulated to make current constant be 1.5A.React after 2 hours, in the gas of generation, synthetic gas content (volume percent) is: 83.38%H
2, 5.81%CO.
Embodiment 4
Respectively by 30gLi
2cO
3, 30gNa
2cO
3, 30gCaCO
3, 46.45gK
2o and 3gNa
2siO
3grind in mortar and mix, be transferred in high purity nickel reactor; Be 20cm by surface-area respectively
2nickel sheet and nickel wire as anode and negative electrode; The spot size of Fresnel Lenses is regulated to make homo(io)thermism be 650 DEG C; The varistor of solar panel circuit is regulated to make current constant be 2A.React after 1 hour, in the gas of generation, synthetic gas content (volume percent) is: 82.28%H
2, 6.11%CO.
Embodiment 5
Respectively by 30gLi
2cO
3, 30gNa
2cO
3, 16.8gCaO and 101.31gRbOH grind and mix in mortar, is transferred in high purity nickel reactor; Be 10cm by surface-area respectively
2nickel sheet and nickel wire as anode and negative electrode; The spot size of Fresnel Lenses is regulated to make homo(io)thermism be 800 DEG C; The varistor of solar panel circuit is regulated to make current constant be 1A.React after 2 hours, in the gas of generation, synthetic gas content (volume percent) is: 80.62%H
2, 6.07%CO.
It is evident that, above description and record be only citing instead of in order to limit content disclosed by the invention, application or use.Under the instruction of the embodiment of the present invention, scope of the present invention will comprise any embodiment of specification sheets and the appended claim fallen into above.
Claims (8)
1. a Driven by Solar Energy high-temperature electrolysis CO
2/ H
2o preparing synthetic gas system, this system comprises electrolysis cells and photo-thermal unit, electrolysis cells is made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen, it is characterized in that: the photovoltaic element of described electrolysis cells converts solar energy into electrical energy, and provides required electrolysis voltage or electric current; Described photo-thermal unit converts solar energy into heat energy, carries out heating and makes it reach molten state, and heat electrolyzer to electrolysis temperature to solid state electrolyte; Described ionogen is the mixture of fused carbonate and fusible hydrate, or the mixture of fused carbonate and molten oxide, or the mixture of fused carbonate, fusible hydrate and molten oxide, in electrolysis, Faradaic current is at [1A, 3A) in interval, electrolyzer temperature is more than 600 DEG C, the CO in electrolyte absorption air
2/ H
2o is regenerated;
When ionogen is the mixture of fused carbonate and fusible hydrate, mol ratio is carbonate: oxyhydroxide=1:0.5 ~ 1; When ionogen is the mixture of fused carbonate and molten oxide, mol ratio is carbonate: oxide compound=1:0.5 ~ 1; When ionogen is the mixture of fused carbonate, fusible hydrate and molten oxide, mol ratio is carbonate: (oxyhydroxide+oxide compound)=1:0.5 ~ 1;
The electrolytic reaction mechanism of this system is:
Anode: 2O
2--4e
-=O
2
Negative electrode: 2OH
-+ CO
3 2-+ 4e
-=CO+H
2+ 4O
2-
2H
++CO
3 2-+4e
-＝CO+H
2+2O
2-。
2. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, is characterized in that, described Faradaic current is 1A-2A, and described electrolyzer temperature is 600 DEG C ~ 800 DEG C.
3. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, is characterized in that, carbonate is Li
2cO
3, Na
2cO
3, K
2cO
3, Rb
2cO
3, MgCO
3, CaCO
3, SrCO
3, BaCO
3, ZnCO
3, Li
2siO
3, Na
2siO
3, K
2siO
3, Rb
2siO
3in one or more mixture; Oxyhydroxide is LiOH, NaOH, KOH, RbOH, Mg (OH)
2, Ca (OH)
2, Sr (OH)
2, Ba (OH)
2, Zn (OH)
2in one or more mixture; Oxide compound is Li
2o, Na
2o, K
2o, Rb
2o, MgO, CaO, SrO, BaO, ZnO, SiO
2, Al
2o
3, Fe
2o
3in one or more mixture.
4. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, it is characterized in that, one in solar cell, nano-crystalline solar battery, dye-sensitized solar battery and concentrating solar battery that described photovoltaic element adopts silicon solar cell plate, multi-band-gap solar cell, functional high molecule material to prepare, or the two or more serial or parallel connection combination in above-mentioned solar cell types.
5. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, it is characterized in that, described photo-thermal unit adopts one or more the combination in Fresnel Lenses, reflection-type beam condenser, refraction type light gathering device, small-sized groove type line-focusing system, dish-style system or tower system, regulates and controls Heating temperature by regulating spot size or focusing ratio.
6. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, is characterized in that, the cathode material of described electrolysis cells is nickel, platinum, titanium, ruthenium, iridium, palladium, iron, tungsten, chromium, copper, gold, graphite or stainless steel, or the alloy of several formation in above-mentioned materials; The anode material of described electrolysis cells is nickel, platinum, titanium, ruthenium, iridium, palladium, iron, tungsten, chromium, copper, gold, graphite or stainless steel, or the alloy of several formation in above-mentioned materials.
7. Driven by Solar Energy high-temperature electrolysis CO according to claim 1
2/ H
2o preparing synthetic gas system, is characterized in that, described electrolyzer adopts high temperature corrosion-resisting type reactor.
8. based on the Driven by Solar Energy high-temperature electrolysis CO one of claim 1-7 Suo Shu
2/ H
2the high-temperature electrolysis CO of O preparing synthetic gas system
2/ H
2the method of O preparing synthetic gas, is characterized in that: the method comprises the steps:
(1) electrolysis cells be made up of photovoltaic element, negative electrode, anode, electrolyzer and ionogen is built;
(2) solid state electrolyte is added in thermal electrolysis to form molten state ionogen by photo-thermal unit;
(3) electrolyzer homo(io)thermism is controlled at 600 DEG C-800 DEG C;
(4) in electrolyzer, CO is passed into by airway
2and H
2o, controls direct supply current constant at 1A-2A, reaction 1h-2h, and main reaction one step generates primary product synthetic gas CO and H
2, main reaction is: CO
2+ H
2o=CO+H
2+ O
2, side reaction obtains intermediate product carbon simple substance and hydrogen, and side reaction is:
1) Formed simple substance the CO that reduces
2/ H
2o generates CO/H
2:
CO
2＝C+O
2
C+CO
2＝2CO
C+H
2O＝H
2+CO
2) water electrolysis generates H
2, H
2reduction CO
2generate CO
H
2O＝H
2+1/2O
2
H
2+CO
2＝CO+H
2O；
Its electrolytic reaction mechanism is:
Anode: 2O
2--4e
-=O
2
Negative electrode: 2OH
-+ CO
3 2-+ 4e
-=CO+H
2+ 4O
2-
2H
++CO
3 2-+4e
-＝CO+H
2+2O
2-。
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